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Rapid Hyperpolarization and Purification of the Metabolite Fumarate in Aqueous Solution

preprint
submitted on 02.09.2020 and posted on 03.09.2020 by Stephan Knecht, John W. Blanchard, Danila Barskiy, Eleonora Cavallari, Laurynas Dagys, Erik van Dyke, Maksim Tsukanov, Bea Bliemel, Kerstin Münnemann, Silvio Aime, Francesca Reineri, Malcolm H. Levitt, Gerd Buntkowsky, Alexander Pines, Peter Blümler, Dmitry Budker, James Eills
Hyperpolarized fumarate is a promising agent for carbon-13 magnetic resonance metabolic imaging of cellular necrosis. Molecular imaging applications require nuclear hyperpolarization to attain sufficient signal strength. Dissolution dynamic nuclear polarization is the current state-of-the-art methodology for hyperpolarizing fumarate, but this is expensive and relatively slow. Alternatively, this important biomolecule can be hyperpolarized in a cheap and convenient manner using parahydrogen-induced polarization. However, this process requires a chemical reaction, and the resulting hyperpolarized fumarate solutions are contaminated with the catalyst, unreacted reagents, and reaction side product molecules, and are hence unsuitable for use in vivo. In this work we show that the hyperpolarized fumarate can be purified from these contaminants by acid precipitation as a pure solid, and later redissolved at a chosen concentration in a clean aqueous solvent. Significant advances in the reaction conditions and reactor equipment allow us to form hyperpolarized fumarate at a concentration of several hundred millimolar, at 13C polarization levels of 30-45%.

Funding

Zero and ultra-low field nuclear magnetic resonance

European Commission

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Functionalized Magnetic Resonance Beacons for Enhanced Spectroscopy and Imaging

European Research Council

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Hyperpolarised MR technologies and molecular probes as alternatives for conventional metal-containing contrast agents for MRI examinations

European Commission

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Athenaeum Research 2016 No. CSTO164550

DFG BU 911/22-2

DFG BU 911/29-1

NSF CHE-1709944

History

Email Address of Submitting Author

eills@uni-mainz.de

Institution

Johannes Gutenberg Universität Mainz

Country

Germany

ORCID For Submitting Author

0000-0001-8468-6860

Declaration of Conflict of Interest

The authors declare no conflict of interest.

Licence

Exports